Periodic nano-structured superlattice with symmetry breaking along the surface as well as thickness is of high importance in plasmonic research due to its immense potential in bio-medical and environmental sensor applications. The structures are rich with electromagnetic hotspots and anisotropic optical properties contributing to the sensitivity of the device. In nanotechnology, nanosphere lithography (NSL) is a promising lithography technique that is in the limelight of research for the last decade due to its simplicity, scalability, and cost-effectiveness. Despite many advantages, the technique is limited in its versatility when it comes to real application. Conventional NSL offers less scope for structural variation with the most common six-fold symmetric structure as the nanosphere mask self-assembles in a hexagonal close-pack fashion due to the very nature of this process. Research efforts have been made to overcome the bottleneck. The conventional NSL approach is modified in combination with other techniques. In this chapter, we discuss the evolution of the NSL technique to achieve maturity. The chapter emphasizes modern NSL formalism associated with techniques like multistep shadow mask deposition and anisotropic etching to achieve 2D and 3D nanostructures with controlled shape, size, inter-structural gap, aspect ratio, sharpness, and special and vertical symmetry. The chapter will serve as an effective knowledge base for further research development in plasmonics, magnonics, and spintronics.